Structural characterisation of molecular conformation and the incorporation of adatoms in an on-surface Ullmann-type reaction.

Structural characterisation of molecular conformation and the incorporation of adatoms in an on-surface Ullmann-type reaction.
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DOI:
10.1038/s42004-020-00402-0
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发表时间:
2020-11-11
影响因子:
5.9
通讯作者:
Saywell, Alex
Saywell, Alex
中科院分区:
化学2区
文献类型:
--
作者:
Judd, Chris J.;Junqueira, Filipe L. Q.;Haddow, Sarah L.;Champness, Neil R.;Duncan, David A.;Jones, Robert G.;Saywell, Alex

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共价键合材料的表面合成在几个方面不同于溶液相合成。从三维反应体积到准二维限制的过渡,如表面合成的情况,有可能促进溶液中可用的替代反应途径。Ullmann型反应,其中表面在芳基卤化物官能化物质的偶联中起作用,已被证明有助于扩展的一维和二维结构。在这里,我们采用扫描隧道显微镜(STM),X-射线光电子能谱(XPS)和X-射线驻波(XSW)分析的组合进行超高真空(UHV)条件下举行的Ag(111)表面上的两个碘功能化物种的Ullmann型耦合的化学和结构表征。我们的研究结果允许表征的分子构象和吸附的几何形状内的表面反应,并提供洞察到反应的中间结构内的金属吸附原子的掺入。金属表面上的Ullmann型反应是表面合成的广泛研究的例子。在这里,结合正常入射的X射线驻波分析,X射线光电子能谱,和扫描隧道显微镜,使在两个这样的反应中的分子构象的表征。
The on-surface synthesis of covalently bonded materials differs from solution-phase synthesis in several respects. The transition from a three-dimensional reaction volume to quasi-two-dimensional confinement, as is the case for on-surface synthesis, has the potential to facilitate alternative reaction pathways to those available in solution. Ullmann-type reactions, where the surface plays a role in the coupling of aryl-halide functionalised species, has been shown to facilitate extended one- and two-dimensional structures. Here we employ a combination of scanning tunnelling microscopy (STM), X-ray photoelectron spectroscopy (XPS) and X-ray standing wave (XSW) analysis to perform a chemical and structural characterisation of the Ullmann-type coupling of two iodine functionalised species on a Ag(111) surface held under ultra-high vacuum (UHV) conditions. Our results allow characterisation of molecular conformations and adsorption geometries within an on-surface reaction and provide insight into the incorporation of metal adatoms within the intermediate structures of the reaction. Ullmann-type reactions on metal surfaces are widely studied examples of on-surface synthesis. Here the combination of normal incidence X-ray standing wave analysis, X-ray photoelectron spectroscopy, and scanning tunneling microscopy enables the characterisation of molecular conformations in two such reactions.
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